Epitaxial Ferroelectric Hf0.5Zr0.5O2 with Metallic Pyrochlore Oxide Electrodes

Zhang, Zimeng; Hsu, Shang‐Lin; Stoica, Vladimir A.; Paik, Hanjong; Parsonnet, Eric; Qualls, Alexander; Wang, Jianjun; Xie, Liang; Kumari, Mukesh; Das, Sujit; Leng, Zhinan; McBriarty, Martin; Proksch, Roger; Gruverman, Alexei; Schlom, Darrell G.; Chen, Long‐Qing; Salahuddin, Sayeef; Martin, Lane W.; Ramesh, Ramamoorthy

doi:10.1002/adma.202006089

Epitaxial Ferroelectric Hf_0.5Zr_0.5O₂ with Metallic Pyrochlore Oxide Electrodes

Journal Article · Tue Feb 02 00:00:00 EST 2021 · Advanced Materials

DOI:https://doi.org/10.1002/adma.202006089· OSTI ID:1806287

^[1]; Hsu, Shang‐Lin ^[2]; Stoica, Vladimir A. ^[3]; Paik, Hanjong ^[4]; Parsonnet, Eric ^[5]; Qualls, Alexander ^[5]; Wang, Jianjun ^[6]; Xie, Liang ^[5]; Kumari, Mukesh ^[5]; Das, Sujit ^[5]; Leng, Zhinan ^[5]; McBriarty, Martin ^[7]; Proksch, Roger ^[8]; Gruverman, Alexei ^[9]; Schlom, Darrell G. ^[10]; Chen, Long‐Qing ^[6]; Salahuddin, Sayeef ^[5]; Martin, Lane W. ^[11]; ^[5]

Univ. of California, Berkeley, CA (United States); Penn State University
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)
Cornell Univ., Ithaca, NY (United States)
Univ. of California, Berkeley, CA (United States)
Pennsylvania State Univ., University Park, PA (United States)
EMD Performance Materials, San Jose, CA (United States)
Asylum Research, Goleta, CA (United States)
Univ. of Nebraska, Lincoln, NE (United States)
Cornell Univ., Ithaca, NY (United States); Kavli Inst. at Cornell for Nanoscale Science, Ithaca, NY (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

The synthesis of fully epitaxial ferroelectric Hf_0.5Zr_0.5O₂ (HZO) thin films through the use of a conducting pyrochlore oxide electrode that acts as a structural and chemical template is reported. Such pyrochlores, exemplified by Pb₂Ir₂O₇(PIO) and Bi₂Ru₂O₇(BRO), exhibit metallic conductivity with room-temperature resistivity of <1 mΩ cm and are closely lattice matched to yttria-stabilized zirconia substrates as well as the HZO layers grown on top of them. Evidence for epitaxy and domain formation is established with X-ray diffraction and scanning transmission electron microscopy, which show that the c-axis of the HZO film is normal to the substrate surface. The emergence of the non-polar-monoclinic phase from the polar-orthorhombic phase is observed when the HZO film thickness is ≥≈30 nm. Furthermore, thermodynamic analyses reveal the role of epitaxial strain and surface energy in stabilizing the polar phase as well as its coexistence with the non-polar-monoclinic phase as a function of film thickness.

View Accepted Manuscript (DOE)

Research Organization:: Pennsylvania State Univ., University Park, PA (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357; SC0012375

OSTI ID:: 1806287

Alternate ID(s):: OSTI ID: 1785882

Journal Information:: Advanced Materials, Journal Name: Advanced Materials Journal Issue: 10 Vol. 33; ISSN 0935-9648

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

References (32)

Atomic Structure of Domain and Interphase Boundaries in Ferroelectric HfO ₂ Grimley, Everett D.; Schenk, Tony; Mikolajick, Thomas Advanced Materials Interfaces, Vol. 5, Issue 5 https://doi.org/10.1002/admi.201701258	journal	January 2018
Water-Splitting Electrocatalysis in Acid Conditions Using Ruthenate-Iridate Pyrochlores Sardar, Kripasindhu; Petrucco, Enrico; Hiley, Craig I. Angewandte Chemie International Edition, Vol. 53, Issue 41 https://doi.org/10.1002/anie.201406668	journal	September 2014
Piezoresponse force microscopy and recent advances in nanoscale studies of ferroelectrics Gruverman, A.; Kalinin, S. V. Journal of Materials Science, Vol. 41, Issue 1 https://doi.org/10.1007/s10853-005-5946-0	journal	January 2006
A new family of bismuth — Precious metal pyrochlores Bouchard, R. J.; Gillson, J. L. Materials Research Bulletin, Vol. 6, Issue 8 https://doi.org/10.1016/0025-5408(71)90100-0	journal	August 1971
Synthesis and physical properties of pyrochlore iridium oxides Pb2$minus;xCaxIr2O7$minus;y Sakai, H. Physica B: Condensed Matter, Vol. 329-333 https://doi.org/10.1016/S0921-4526(02)02239-1	journal	May 2003
Direct Epitaxial Growth of Polar (1 – x )HfO ₂ –( x )ZrO ₂ Ultrathin Films on Silicon Nukala, Pavan; Antoja-Lleonart, Jordi; Wei, Yingfen ACS Applied Electronic Materials, Vol. 1, Issue 12 https://doi.org/10.1021/acsaelm.9b00585	journal	November 2019
Piezoresponse force microscopy and nanoferroic phenomena Gruverman, Alexei; Alexe, Marin; Meier, Dennis Nature Communications, Vol. 10, Issue 1 https://doi.org/10.1038/s41467-019-09650-8	journal	April 2019
A rhombohedral ferroelectric phase in epitaxially strained Hf0.5Zr0.5O2 thin films Wei, Yingfen; Nukala, Pavan; Salverda, Mart Nature Materials, Vol. 17, Issue 12 https://doi.org/10.1038/s41563-018-0196-0	journal	October 2018
Enhanced ferroelectricity in ultrathin films grown directly on silicon Cheema, Suraj S.; Kwon, Daewoong; Shanker, Nirmaan Nature, Vol. 580, Issue 7804 https://doi.org/10.1038/s41586-020-2208-x	journal	April 2020
Charting the complete elastic properties of inorganic crystalline compounds de Jong, Maarten; Chen, Wei; Angsten, Thomas Scientific Data, Vol. 2, Issue 1 https://doi.org/10.1038/sdata.2015.9	journal	March 2015
The demonstration of significant ferroelectricity in epitaxial Y-doped HfO2 film Shimizu, Takao; Katayama, Kiliha; Kiguchi, Takanori Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/srep32931	journal	September 2016
Surface and grain boundary energy as the key enabler of ferroelectricity in nanoscale hafnia-zirconia: a comparison of model and experiment Park, Min Hyuk; Lee, Young Hwan; Kim, Han Joon Nanoscale, Vol. 9, Issue 28 https://doi.org/10.1039/C7NR02121F	journal	January 2017
Understanding the formation of the metastable ferroelectric phase in hafnia–zirconia solid solution thin films Park, Min Hyuk; Lee, Young Hwan; Kim, Han Joon Nanoscale, Vol. 10, Issue 2 https://doi.org/10.1039/C7NR06342C	journal	January 2018
Depolarization fields in thin ferroelectric films Mehta, R. R.; Silverman, B. D.; Jacobs, J. T. Journal of Applied Physics, Vol. 44, Issue 8 https://doi.org/10.1063/1.1662770	journal	August 1973
Ferroelectricity in hafnium oxide thin films Böscke, T. S.; Müller, J.; Bräuhaus, D. Applied Physics Letters, Vol. 99, Issue 10 https://doi.org/10.1063/1.3634052	journal	September 2011
Evolution of phases and ferroelectric properties of thin Hf _0.5 Zr _0.5 O ₂ films according to the thickness and annealing temperature Hyuk Park, Min; Joon Kim, Han; Jin Kim, Yu Applied Physics Letters, Vol. 102, Issue 24 https://doi.org/10.1063/1.4811483	journal	June 2013
The effects of crystallographic orientation and strain of thin Hf _0.5 Zr _0.5 O ₂ film on its ferroelectricity Hyuk Park, Min; Joon Kim, Han; Jin Kim, Yu Applied Physics Letters, Vol. 104, Issue 7 https://doi.org/10.1063/1.4866008	journal	February 2014
The origin of ferroelectricity in Hf _1−x Zr _x O ₂ : A computational investigation and a surface energy model Materlik, R.; Künneth, C.; Kersch, A. Journal of Applied Physics, Vol. 117, Issue 13 https://doi.org/10.1063/1.4916707	journal	April 2015
On the structural origins of ferroelectricity in HfO ₂ thin films Sang, Xiahan; Grimley, Everett D.; Schenk, Tony Applied Physics Letters, Vol. 106, Issue 16 https://doi.org/10.1063/1.4919135	journal	April 2015
Growth of epitaxial orthorhombic YO _1.5 -substituted HfO ₂ thin film Shimizu, Takao; Katayama, Kiliha; Kiguchi, Takanori Applied Physics Letters, Vol. 107, Issue 3 https://doi.org/10.1063/1.4927450	journal	July 2015
Large ferroelectric polarization of TiN/Hf _0.5 Zr _0.5 O ₂ /TiN capacitors due to stress-induced crystallization at low thermal budget Kim, Si Joon; Narayan, Dushyant; Lee, Jae-Gil Applied Physics Letters, Vol. 111, Issue 24 https://doi.org/10.1063/1.4995619	journal	December 2017
Local polarization dynamics in ferroelectric materials Kalinin, Sergei V.; Morozovska, Anna N.; Chen, Long Qing Reports on Progress in Physics, Vol. 73, Issue 5, Article No. 056502 https://doi.org/10.1088/0034-4885/73/5/056502	journal	April 2010
Dual-frequency resonance-tracking atomic force microscopy Rodriguez, Brian J.; Callahan, Clint; Kalinin, Sergei V. Nanotechnology, Vol. 18, Issue 47, Article No. 475504 https://doi.org/10.1088/0957-4484/18/47/475504	journal	October 2007
Relative stability of ZrO 2 and HfO 2 structural phases Lowther, J. E.; Dewhurst, J. K.; Leger, J. M. Physical Review B, Vol. 60, Issue 21 https://doi.org/10.1103/PhysRevB.60.14485	journal	December 1999
Electron interactions, spin-orbit coupling, and intersite correlations in pyrochlore iridates Wang, Runzhi; Go, Ara; Millis, Andrew J. Physical Review B, Vol. 95, Issue 4 https://doi.org/10.1103/PhysRevB.95.045133	journal	January 2017
Polarization Relaxation Induced by a Depolarization Field in Ultrathin Ferroelectric BaTiO 3 Capacitors Kim, D. J.; Jo, J. Y.; Kim, Y. S. Physical Review Letters, Vol. 95, Issue 23 https://doi.org/10.1103/PhysRevLett.95.237602	journal	December 2005
Bismuth-Ruthenate-Based Cathodes for IT-SOFCs Jaiswal, Abhishek; Wachsman, Eric D. Journal of The Electrochemical Society, Vol. 152, Issue 4 https://doi.org/10.1149/1.1866093	journal	January 2005
Applicability of Bi[sub 2]Ru[sub 2]O[sub 7] Pyrochlore Electrodes for ESB and BIMEVOX Electrolytes Esposito, Vincenzo; Luong, Bac H.; Di Bartolomeo, Elisabetta Journal of The Electrochemical Society, Vol. 153, Issue 12 https://doi.org/10.1149/1.2358088	journal	January 2006
(Invited) Epitaxial HfO ₂ Thin Films on Si Substrates: Strategy for Sub-1 nm EOT Technology Migita, Shinji; Ota, Hiroyuki ECS Transactions, Vol. 41, Issue 3 https://doi.org/10.1149/1.3633029	journal	October 2011
Rotating Disk Electrode Voltammetry of Thin Films of Novel Oxide Materials Wakabayashi, Ryo H.; Paik, Hanjong; Murphy, Marc J. Journal of The Electrochemical Society, Vol. 164, Issue 14 https://doi.org/10.1149/2.1021714jes	journal	January 2017
A fast image simulation algorithm for scanning transmission electron microscopy Ophus, Colin Advanced Structural and Chemical Imaging, Vol. 3, Issue 1 https://doi.org/10.1186/s40679-017-0046-1	journal	May 2017
A streaming multi-GPU implementation of image simulation algorithms for scanning transmission electron microscopy Pryor, Alan; Ophus, Colin; Miao, Jianwei Advanced Structural and Chemical Imaging, Vol. 3, Issue 1 https://doi.org/10.1186/s40679-017-0048-z	journal	October 2017

Similar Records

Engineering Ferroelectric Hf_0.5Zr_0.5O₂ Thin Films by Epitaxial Stress

Journal Article · Tue Jul 02 20:00:00 EDT 2019 · ACS Applied Electronic Materials · OSTI ID:2572166

Unraveling Ferroelectric Polarization and Ionic Contributions to Electroresistance in Epitaxial Hf_0.5Zr_0.5O₂ Tunnel Junctions

Journal Article · Wed Nov 13 19:00:00 EST 2019 · Advanced Electronic Materials · OSTI ID:1606631

Related Subjects

36 MATERIALS SCIENCE
epitaxial growth
ferroelectrics
hafnia

Epitaxial Ferroelectric Hf0.5Zr0.5O2 with Metallic Pyrochlore Oxide Electrodes

Citation Formats

References (32)

Similar Records

Related Subjects

Epitaxial Ferroelectric Hf_0.5Zr_0.5O₂ with Metallic Pyrochlore Oxide Electrodes